We report multifunctional tendon-mimetic hydrogels constructed from anisotropic assembly of aramid nanofiber composites. The stiff nanofibers and soft polyvinyl alcohol in these anisotropic composite hydrogels (ACHs) mimic the structural interplay between aligned collagen fibers and proteoglycans in tendons. The ACHs exhibit a high modulus of ~1.1 GPa, strength of ~72 MPa, fracture toughness of 7333 J/m2, and many additional characteristics matching those of natural tendons, which was not achieved with previous synthetic hydrogels. The surfaces of ACHs were functionalized with bioactive molecules to present biophysical cues for the modulation of morphology, phenotypes, and other behaviors of attached cells. Moreover, soft bioelectronic components can be integrated on ACHs, enabling in situ sensing of various physiological parameters. The outstanding mechanics and functionality of these tendon mimetics suggest their further applications in advanced tissue engineering, implantable prosthetics, human-machine interactions, and other technologies.